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Facile synthesis of accordion-like porous carbon from waste PET bottles-based MIL-53(Al) and its application for high-performance Zn-ion capacitor

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Green Energy & Environment 2024年第7期9卷 1138-1150页

作者： Jiaxin Li Shuai Zhang Yumeng Hua Yichao Lin Xin Wen Ewa Mijowska Tao Tang Xuecheng Chen Rodney S.Ruoff Faculty of Chemical Technology and engineering West Pomeranian University of Technology key State key laboratory of Polymer Physics and Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of Safety engineering China University of Mining and Technology Institute of Advanced Electrical Materials Qingdao University of Science and Technology Institute for Basic Science Center for Multiple Dimensional carbon Materials Department of Chemistry Ulsan National Institute of Science and Technology (UNIST) Department of Materials Science and engineering Ulsan National Institute of Science and Technology (UNIST) School of Energy and Chemical engineering Ulsan National Institute of Science and Technology (UNIST)

It is of great scientific and economic value to recycle waste poly（ethylene terephthalate）(PET) into high-value PET-based metal organic frameworks（MOFs） and further convert it into porous carbon for green energy storage applications. In the present study, a facile and costeffective hydrothermal process was developed to direct recycle waste PET bottles into MIL-53（Al） with a 100% conversation, then the MOFderived porous carbon was assembled into electrodes for high-performance supercapacitors. The results indicated that the as-synthesized carbon exhibited high SSA of 1712 m2g-1and unique accordion-like structure with hierarchical porosity. Benefit to these advantageous characters, the assembled three-electrode supercapacitor displayed high specific capacitances of 391 F g-1at the current density of 0.5 A g-1and good rate capability of 73.6% capacitance retention at 20 A g-1in 6 mol L-1KOH electrolyte. Furthermore, the assembled zinc ion capacitor still revealed outstanding capacitance of 335 F g-1at 0.1 A g-1, excellent cycling stability of 92.2% capacitance retention after 10 000 cycles and ultra-high energy density of 150.3 Wh kg-1at power density of 90 W kg-1in 3 mol L-1ZnSO4electrolyte. It is believed that the current work provides a facile and effective strategy to recycle PET waste into high-valuable MOF, and further expands the applications of MOF-derived carbons for high-performance energy storage devices, so it is conducive to both pollution alleviation and sustainable economic development.

关键词： PET Recycling Porous carbon Supercapacitor Energy storage

Constructing a 3D multichannel structure to enhance performance of Ni–Co–Mn hydroxide electrodes for flexible supercapacitors

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Rare Metals 2024年第1期43卷 148-163页

作者： Zhi-Hui Xu Shi-Shuai Sun Xue-Lei Li Zhi-Hui Zhang Hai-Ying Li Shuang-Ting Ruan Shou-Gen Yin key laboratory of Display Materials and Photoelectric Devices(Ministry of Education)and Tianjin key laboratory for Photoelectric Materials and Devices School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China College of Science Tianjin University of TechnologyTianjin 300384China School of Materials Science and engineering Inner Mongolia University of TechnologyHohhot 010051China

The balancing of the electrochemical performance,mechanical stability,and processing technology for applying supercapacitors to flexible and wearable electronics continues to encounter severe ***,we prepare Ni-Co-Mn hydroxide electrodes with a threedimensional multichannel structure via a simple hydrothermal *** are constructed using vertically contiguous nano sheets with a uniform thickness and rough *** electrodes can provide numerous electroactive sites and accelerate the transmission of electrolyte *** relationship between the structure and electrochemical performances is verified by experiments and theoretical ***-dimensional(2D)planar and one-dimensional(1D)fiber electrodes are prepared using a flexible carbon cloth(CC)and carbon fiber(CF),respectively,as *** assembled quasi-solid-state flexible asymmetric supercapacitor(FASC)with a twodimensional sandwich structure using NiCoMn-OH/CC as the electrode achieves a remarkable energy density of73.8 Wh·kg^(-1)at a power density of 1.03 kW·kg^(-1).The quasi-solid-state FASC with a 1D linear structure using NiCoMn-OH/CF as the electrode also attains a high energy density(12.9 Wh·kg^(-1)at a power density of0.75 W·kg^(-1)).Moreover,the electrochemical performances of the NiCoMn/CC//AC/CC and NiCoMn/CF//AC/CF FASCs are not disturbed at different bending angles(0°,45°,90°,135°and 180°),This indicates the superior flexibility of the *** also assemble a self-powered energy-harvesting storage system by integrating FASCs and commercial solar cells to verify its *** displays sustainable development potential for energy storage.

关键词： Supercapacitors Flexible Ni–Co–Mn hydroxide 3D multichannel structure High performances

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engineering catalytic defects via molecular imprinting for high energy Li-S pouch cells

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National Science Review 2024年第07期 239-251页

作者： Yufei Zhao Chuannan Geng Li Wang Yun Cao Haotian Yang Linkai Peng Xin Jiang Yong Guo Xiaolin Ye Wei Lv Quan-Hong Yang Shenzhen Geim Graphene Center Engineering Laboratory for Functionalized Carbon Materials Tsinghua Shenzhen International Graduate School Tsinghua University Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy StorageSchool of Chemical Engineering and Technology and Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin University Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University

Heterogeneous catalysis promises to accelerate sulfur-involved conversion reactions in lithium-sulfur batteries. Solid-state Li2S dissociation remains as the rate-limiting step because of the weakly matched solid-solid electrocatalysis interfaces. We propose an electrochemically molecular-imprinting strategy to have a metal sulfide（MS） catalyst with imprinted defects in positions from which the pre-implanted Li2S has been electrochemically removed. Such tailor-made defects enable the catalyst to bind exclusively to Li atoms in Li2S reactant and elongate the Li–S bond, thus decreasing the reaction energy barrier during charging. The imprinted Ni3S2catalyst shows the best activity due to the highest defect concentration among the MS catalysts examined. The Li2S oxidation potential is substantially reduced to 2.34 V from 2.96 V for the counterpart free of imprinted vacancies, and an Ah-level pouch cell is realized with excellent cycling performance. With a lean electrolyte/sulfur ratio of 1.80 μL mgS–1, the cell achieves a benchmarkedly high energy density beyond 500 Wh kg–1.

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Crystal facet-dependent CO_(2) cycloaddition to epoxides over ZnO catalysts

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Frontiers of Chemical Science and engineering 2024年第5期18卷 49-59页

作者： Yongjian Wei Ying Li Yunfei Xu Yinghui Sun Tong Xu Haiou Liang Jie Bai Inner Mongolia key laboratory of Industrial Catalysis Hohhot 010051China College of Chemical engineering Inner Mongolia University of TechnologyHohhot 010051China

With regard to green chemistry and sustainable development,the fixation of CO_(2) into epoxides to form cyclic carbonates is an attractive and promising pathway for CO_(2) *** oxides,renowned as promising eco-friendly catalysts for industrial production,are often undervalued in terms of their impact on the CO_(2)addition *** this work,we successfully developed ZnO nanoplates with(002)surfaces and ZnO nanorods with(100)surfaces via morphology-oriented regulation to explore the effect of crystal faces on CO_(2) *** quantitative data obtained from electron paramagnetic resonance spectroscopy indicated that the concentration of oxygen vacancies on the ZnO nanoplate surfaces was more than twice that on the ZnO nanorod *** functional theory calculations suggested that the(002)surfaces have lower adsorption energies for CO_(2) and epichlorohydrin than the(100)*** a result,the yield of cyclochloropropene carbonate on the ZnO nanoplates(64.7%)was much greater than that on the ZnO nanorods(42.3%).Further evaluation of the reused catalysts revealed that the decrease in the oxygen vacancy concentration was the primary factor contributing to the decrease in catalytic *** on these findings,a possible catalytic mechanism for CO_(2) cycloaddition with epichlorohydrin was *** work provides a new idea for the controllable preparation of high-performance ZnO catalysts for the synthesis of cyclic carbonates from CO_(2) and epoxides.

关键词： carbon dioxide cycloaddition zinc oxide crystal face oxygen vacancy

Non-bonding modulations between single atomic cerium and monodispersed selenium sites towards efficient oxygen reduction

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Nano Research 2024年第6期17卷 4753-4763页

作者： Leilei Yin Shuai Zhang Mingzi Sun Siyuan Wang Bolong Huang Yaping Du Tianjin key Lab for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin 300350China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina Research Centre for carbon-Strategic Catalysis The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina

Currently,dual atomic catalysts(DACs)with neighboring active sites for oxygen reduction reaction(ORR)still meet lots of challenges in the synthesis,especially the construction of atomic pairs of elements from different blocks of the periodic ***,a“rare earth(Ce)-metalloid(Se)”non-bonding heteronuclear diatomic electrocatalyst has been constructed for ORR by rational coordination and carbon support defect ***,the optimized Ce-Se diatomic catalysts(Ce-Se DAs/NC)displayed a half-wave potential of 0.886 V *** hydrogen electrode(RHE)and excellent stability,which surpass those of separate Ce or Se single atoms and most single/dual atomic catalysts ever *** addition,a primary zinc-air battery constructed using Ce-Se DAs/NC delivers a higher peak power density(209.2 mW·cm^(−2))and specific capacity(786.4 mAh·gZn^(−1))than state-of-the-art noble metal catalysts Pt/*** calculations reveal that the Ce-Se DAs/NC has improved the electroactivity of the Ce-N_(4)region due to the electron transfer towards the nearby Se specific activity(SA)***,the more electron-rich Se sites promote the adsorptions of key intermediates,which results in the optimal performances of ORR on Ce-Se DAs/*** work provides new perspectives on electronic structure modulations via non-bonded long-range coordination micro-environment engineering in DACs for efficient electrocatalysis.

关键词： catalyst rare earth oxygen reduction reaction(ORR) metalloid non-bonding modulation

Breakthrough of carbon-Ash Recalcitrance in Hydrochar via Molten carbonate:engineering Mineral-Rich Biowaste Toward sustainable Platform carbon Materials

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engineering 2024年第5期36卷 167-177页

作者： Zihan Wang Leli Zhang Yuanhui Zhang Zhidan Liu laboratory of Environment-Enhancing Energy(E2E) Key Laboratory of Agricultural Engineering in Structure and EnvironmentMinistry of AgricultureCollege of Water Resources and Civil EngineeringChina Agricultural UniversityBeijing 100083China Department of Agricultural and Biological engineering University of Illinois at Urbana-ChampaignUrbanaIL 61801USA

The function-led design of porous hydrochar from mineral-rich biowaste for environmental applications inevitably suffers from carbon-ash ***,a method to alter the original carbon skeleton with ash remains elusive and hinders the availability of ***,we propose a facile strategy for breaking the rigid structure of carbon-ash coupled hydrochar using phase-tunable molten carbonates.A case system was designed in which livestock manure and NaHCO3 were used to prepare the activated hydrochar,and NH3 served as the target *** to the redox effect,we found that organic fractions significantly advanced the melting temperature of Na2CO3 below 800℃.The Na species steadily broke the carbon-ash interaction as the thermal intensity increased and transformed inorganic constituents to facilitate ash dissolution,rebuilding the hydrochar skeleton with abundant hierarchical channels and active defect *** surface polarity and mesopore distribution collectively governed the five cycles NH3 adsorption attenuation *** hydrochar delivered favorable potential for application with a maximum overall adsorption capacity of 100.49 mg·g^(-1).Integrated spectroscopic characterization and theoretical computations revealed that incorporating NH3 on the carbon surface could transfer electrons to chemisorbed oxygen,which promoted the oxidation of pyridine-N during *** work offers deep insight into the structure function correlation of hydrochar and inspires a more rational design of engineered hydrochar from high-ash biowaste.

关键词： Hydrochar Livestock manure Ammonia adsorption Deashing Oxygen activation

Roadmap for rechargeable batteries:present and beyond

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Science China Chemistry 2024年第1期67卷 13-42页

作者： Sen Xin Xu Zhang Lin Wang Haijun Yu Xin Chang Yu-Ming Zhao Qinghai Meng Pan Xu Chen-Zi Zhao Jiahang Chen Huichao Lu Xirui Kong Jiulin Wang Kai Chen Gang Huang Xinbo Zhang Yu Su Yao Xiao Shu-Lei Chou Shilin Zhang Zaiping Guo Aobing Du Guanglei Cui Gaojing Yang Qing Zhao Liubing Dong Dong Zhou Feiyu Kang Hu Hong Chunyi Zhi Zhizhang Yuan Xianfeng Li Yifei Mo Yizhou Zhu Dongfang Yu Xincheng Lei Jianxiong Zhao Jiayi Wang Dong Su Yu-Guo Guo Qiang Zhang Jun Chen Li-Jun Wan CAS key laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences.Beijing 100049 China Institute of Advanced Battery Materials and Devices Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China key laboratory of Advanced Functional Materials Ministry of EducationBeijing University of TechnologyBeijing 100124China Beijing key laboratory of Green Chemical Reaction engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China State key laboratory of Chemistry and Utilization of carbon-Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830046China Department of Chemical engineering Shanghai Jiao Tong UniversityShanghai 200240China State key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChangchun 130022China Institute for carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China School of Chemical engineering and Advanced Materials The University of AdelaideAdelaide 5000Australia Qingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China Frontiers Science Center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China College of Chemistry and Materials Science Jinan UniversityGuangzhou 511443China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhen 518055China Department of Materials Science and engineering City University of Hong KongHong Kong 999077China Division of Energy Storage Dalian National Laboratory for Clean Energy(DNL)Dalian Institute of Chem

Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate *** to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable *** efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow *** the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a *** roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable *** computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.

关键词： energy storage rechargeable batteries battery materials electrochemistry

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MOF-mediated synthesis of novel PtFeCoNiMn high-entropy nanoalloy as bifunctional oxygen electrocatalysts for zinc-air battery

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Nano Research 2024年第6期17卷 5288-5297页

作者： Mingkuan Xie Xin Xiao Duojie Wu Cheng Zhen Chunsheng Wu Wenjuan Wang Hao Nian Fayan Li Meng Danny Gu Qiang Xu Shenzhen key laboratory of Micro/Nano-Porous Functional Materials(SKLPM) Shenzhen 518055China Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China Department of Materials Science and engineering Southern University of Science and TechnologyShenzhen 518055China SUSTech-Kyoto University Advanced Energy Materials Joint Innovation laboratory(SKAEM-JIL) Shenzhen 518055China key University laboratory of Highly Efficient Utilization of Solar Energy and sustainable Development of Guangdong Southern University of Science and TechnologyShenzhen 518055China Eastern Institute for Advanced Study Eastern Institute of TechnologyNingbo 315200China

High-entropy alloy(HEA)-based materials are expected to be promising oxygen electrocatalysts due to their exceptional *** electronic structure regulation of HEAs plays a pivotal role in enhancing their elctrocatalytic ***,PtFeCoNiMn nanoparticles(NPs)with subtle lattice distortions are constructed on metal-organic framework-derived nitrogen-doped carbon by an ultra-rapid Joule heating *** to the modulated electronic structure and the inherent cocktail effect of HEAs,the as-synthesized PtFeCoNiMn/NC exhibits superior bifunctional electrocatalytic performance with a positive half-wave potential of 0.863 V *** hydrogen electrode(RHE)for oxygen reduction reaction and a low overpotential of 357 mV at 10 mA·cm^(-2)for oxygen evolution *** assembled quasi-solid-state zinc-air battery using PtFeCoNiMn/NC as air electrode shows a high peak power density of 192.16 mW·cm^(-2),low charge−discharge voltage gap,and excellent durability over 500 cycles at 5 mA·cm^(-2).This work demonstrates an effective route for rational design of bifunctional nanostructured HEA electrocatalysts with favorable electronic structures,and opens up a fascinating directions for energy storage and conversion,and beyond.

关键词： oxygen reduction reaction oxygen evolution reaction high-entropy nano-alloy zinc-air battery

Valorization of carbon dioxide with alcohols

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Chinese Chemical Letters 2024年第7期35卷 54-58页

作者： Daheng Wen Weiwei Fang Yongmei Liu Tao Tu Shanghai key laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing 210037China State key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Utilizing CO_(2)for the production of bulky and valuable chemicals presents an attractive solution to address environmental and fossil energy *** the various approaches,direct carboxylation of alcohols with CO_(2)stands out as an eco-friendly process capable of efficiently producing carboxylic acids in a sustainable ***,the high dissociation energy of the C–O bond poses a significant challenge in this *** the past few decades,several strategies have been developed to activate alcohols and establish efficient catalytic systems for carboxylation with CO_(2).Nevertheless,the sporadic nature of reported approaches makes it difficult to determine the most effective *** perspective aims to provide an overview of the current state-of-the-art catalytic protocols for carboxylating alcohols with CO_(2),encompassing esterification,halogenation,and photocatalysis,while considering their respective advantages and *** aim to discern the most promising avenues for future development in this *** insights presented in this perspective will contribute to the advancement of efficient and sustainable carboxylation methods using CO_(2),leading to the production of valuable chemicals in future.

关键词： Carboxylation carbon dioxide Alcohol Carboxylic acid Transition metal catalysis

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